Zirconium Carbide Mediates Coke‐Resistant Methane Dry Reforming on Nickel‐Zirconium Catalysts

Graphitic deposits anti‐segregate into Ni0 nanoparticles to provide restored CH4 adsorption sites and near‐surface/dissolved C atoms, which migrate to the Ni0/ZrO2 interface and induce local ZrxCy formation. The resulting oxygen‐deficient carbidic phase boundary sites assist in the kinetically enhan...

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Bibliographic Details
Published in:Angewandte Chemie (International ed.) 2022-12, Vol.61 (50), p.e202213249-n/a
Main Authors: Haug, Leander, Thurner, Christoph, Bekheet, Maged F., Bischoff, Benjamin, Gurlo, Aleksander, Kunz, Martin, Sartory, Bernhard, Penner, Simon, Klötzer, Bernhard
Format: Article
Language:English
Subjects:
Carbon dioxide
Carbon Spillover
Catalysts
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Methane
Methane Dry Reforming
Nanoparticles
Near Ambient Pressure XPS
Nickel
NiZr Intermetallic Catalyst
Oxygen
Reforming
Zirconium
Zirconium Carbide
Zirconium dioxide
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Summary:Graphitic deposits anti‐segregate into Ni0 nanoparticles to provide restored CH4 adsorption sites and near‐surface/dissolved C atoms, which migrate to the Ni0/ZrO2 interface and induce local ZrxCy formation. The resulting oxygen‐deficient carbidic phase boundary sites assist in the kinetically enhanced CO2 activation toward CO(g). This interface carbide mechanism allows for enhanced spillover of carbon to the ZrO2 support, and represents an alternative catalyst regeneration pathway with respect to the reverse oxygen spillover on Ni‐CeZrxOy catalysts. It is therefore rather likely on supports with limited oxygen storage/exchange kinetics but significant carbothermal reducibility. Zr‐Carbide promoted Methane Dry Reforming on NixZry: Graphitic deposits anti‐segregate into Ni0 nanoparticles to provide restored CH4 adsorption sites and near‐surface/dissolved C atoms, which migrate toward the Ni0/ZrO2 interface and induce local ZrxCy formation. The resulting oxygen‐deficient carbidic phase boundary sites assist in kinetically enhanced CO2 activation toward CO(g).
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202213249